The dynamic anti-corrosion of self-derived space charge layer enabling long-term stable seawater oxidation

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-24 DOI:10.1016/j.apcatb.2023.123658
Jie Zhu , Baoguang Mao , Bo Wang, Minhua Cao
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Abstract

Developing corrosion-resistant oxygen evolution electrocatalysts that can sustain seawater electrolysis is crucial but challenging for hydrogen production. Herein, we develop a bimetallic oxyhydroxide electrocatalyst with self-derived selenate space charge layer (SeO42− SCL) by in-situ electrochemically reconstructing cobalt-doped nickel diselenide (Co-NiSe2) pre-catalyst, enabling long-term stability for seawater electrolysis. In-situ experiments and theoretical results reveal the promoting effect of cobalt-doping on the reconstruction of NiSe2 and generation of dynamically stable oxygen vacancy sites. Importantly, the SeO42− SCL derived from the reconstruction process shows a dynamic anti-corrosion behavior, thus protecting metal species from dissolution and meanwhile without blocking the diffusion and adsorption of reactive species. Consequently, a two-electrode cell assembled by this Co-NiSe2 pre-catalyst as an anode, reaches an industrial current density (500 mA cm−2) at a cell voltage of 1.70 V, and that works stably for over 1500 h in alkaline seawater, which is of significance for promoting the practicality of low-cost catalysts.

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实现海水长期稳定氧化的自衍生空间电荷层的动态抗腐蚀能力
开发可维持海水电解的耐腐蚀氧进化电催化剂对于制氢至关重要,但也极具挑战性。在此,我们通过对掺钴二硒化镍(Co-NiSe2)前催化剂进行原位电化学重构,开发出一种具有自生硒酸空间电荷层(SeO42- SCL)的双金属氢氧化物电催化剂,从而实现了海水电解的长期稳定性。原位实验和理论结果表明,钴掺杂对 NiSe2 的重构和动态稳定氧空位的生成具有促进作用。重要的是,重构过程中产生的 SeO42- SCL 具有动态抗腐蚀性能,从而保护金属物种免受溶解,同时不会阻碍活性物种的扩散和吸附。因此,以这种 Co-NiSe2 前催化剂为阳极组装的双电极电池在电池电压为 1.70 V 时达到了工业电流密度(500 mA/cm2),并能在碱性海水中稳定工作 1500 小时以上,这对促进低成本催化剂的实用化具有重要意义。
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来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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